【摘要】 非晶纳米材料因长程无序的原子排列,其形貌和结构的调控极具挑战性.本文首次报道了一种可控自水解蚀刻-沉淀（SHEP）法,在常温常压下即可合成出空心多孔且形貌规则的非晶Cu2MoS4纳米笼（a-Cu₂MoS₄）.得益于其空心多孔结构和非晶的丰富硫缺陷,a-Cu2MoS4表现出比晶体相对物更强的析氢反应（HER）活性.其中,壳厚度为20 nm的八面体a-Cu2MoS4表现出最好的HER活性:在10 mA cm^-2电流密度下,过电位仅为96 mV,塔菲尔斜率低至61 mV decade^-1;这主要是因为a-Cu2MoS4合适的厚度既保证了其表面的多孔性,又确保了其结构的稳定性.本文提出的合成方法具有普适性,可扩展到更多的三元纳米笼材料的合成,为各种三元纳米笼的精确可控制备提供了新视角,并为开发高活性非晶催化剂开辟了新的途径.更多还原

【Abstract】 Morphological and structural control of amorphous nanomaterials is challenging due to the long-range disordered atomic arrangements. Herein, we firstly propose a controllable self-hydrolyzing etching-precipitating（SHEP）method to fabricate the regular-shaped amorphous Cu₂ MoS₄ nanocages（a-Cu₂ MoS₄ NCs） with hollow porous structures under ambient conditions. Benefitting from the hollow porous structures and the amorphous characteristics with copious sulfur vacancies, the a-Cu₂ MoS₄ NCs possess more enhanced activity toward hydrogen evolution reaction（HER） than their crystalline counterparts. The octahedral a-Cu₂ MoS₄ NCs with a shell thickness of 20 nm, which balance the appropriate surface porosity and good structural stability, exhibit the best HER activity with a low overpotential of 96 mV at 10 mA cm^-2 and a small tafel slope of 61 mV decade^-1 in alkaline environment. Moreover, this method is very versatile and can be extended to synthesize other ternary nanocages. Our current work may shed light on the precise controllable synthesis of various ternary nanocages and open a new frontier for developing highly active amorphous catalysts.更多还原